Korean Journal of Environmental Agriculture (한국환경농학회지)

The Korean Society of Environmental Agriculture (한국환경농학회)
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Development of Simultaneous Analytical Method of Veterinary Antibiotics in Manure using Liquid Chromatography Coupled with Tandem Mass Spectrometry

LC-MS/MS를 이용한 퇴비 및 액비 중 항생제 동시 분석법 개발

  • Chung, Hyung Suk (Division of Applied Bioscience and Biotechnology, College of Agriculture and Life Sciences, Chonnam National University) ;
  • Lee, Young Jun (Kyung Nong Co., Ltd., Central Research Institute) ;
  • Lee, Han Sol (Division of Applied Bioscience and Biotechnology, College of Agriculture and Life Sciences, Chonnam National University) ;
  • Rahman, Md. Musfiqur (Division of Applied Bioscience and Biotechnology, College of Agriculture and Life Sciences, Chonnam National University) ;
  • Kabir, Md. Humayun (Division of Applied Bioscience and Biotechnology, College of Agriculture and Life Sciences, Chonnam National University) ;
  • Park, Byung-Jun (Chemical Safety Division, Department of Agro-Food Safety and Crop Protection, National Institute of Agricultural Science) ;
  • Kim, Jang-Eok (School of Applied Biosciences, College of Agriculture and Life Sciences, Kyungpook National University) ;
  • Shim, Jae-Han (Division of Applied Bioscience and Biotechnology, College of Agriculture and Life Sciences, Chonnam National University)
  • 정형석 (전남대학교 농업생명과학대학 농식품생명화학부) ;
  • 이영준 (경농 중앙연구소 안전성연구팀) ;
  • 이한솔 (전남대학교 농업생명과학대학 농식품생명화학부) ;
  • ;
  • ;
  • 박병준 (국립농업과학원 농산물안전성부 화학물질안전과) ;
  • 김장억 (경북대학교 농업생명과학대학 응용생명과학부) ;
  • 심재한 (전남대학교 농업생명과학대학 농식품생명화학부)
  • Received : 2017.06.22
  • Accepted : 2017.09.19
  • Published : 2017.09.30
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Abstract

BACKGROUND: The current study was to monitor of 9 veterinary antibiotics (ceftiofur, clopidol, florfenicol, sulfamethazine, sulfamethoxazole, sulfathiazole, tetracycline, tiamulin, and tylosin) in manure using liquid chromatography-tandem mass spectrometry (LC-MS/MS) in positive and negative electrospray ionization mode. METHODS AND RESULTS: Sample preparation was carried out using Mcllvaine buffer and citrate salts to adjust the pH of the sample followed by purification with dispersive solid phase extraction (d-SPE). Separation of analytes during LC-MS/MS analysis was conducted using an Eclipse Plus $C_{18}$ column and the mobile phase was in gradient mode with, 0.1% formic acid and 5 mM ammonium formate in methanol (A) and 0.1% formic acid and 5 mM ammonium formate in distilled water (B). The linearity of the matrix-matched calibrations of all tested antibiotics was good, with $R^2$ determination coefficients ${\geq}0.9920$. The limit of detection (LOD) and quantifications (LOQ) were $0.1-67.0{\mu}g/kg$ and $0.4-200.0{\mu}g/kg$, respectively. Analysis of 13 solid and liquid manure samples taken from the Republic of Korea revealed concentrations less than $0.7{\mu}g/kg$ for tiamulin, $1497.6{\mu}g/kg$ for sulfamethazine. CONCLUSION: To monitor 9 veterinary antibiotics from manure samples in 13 provincial areas throughout the Republic of Korea, an analytical method was developed. The developed method was fully validated and successfully applied for monitoring various veterinary antibiotics in manure samples.

전국의 퇴비 및 액비 시료에서 대상 항생제 종9 (ceftiofur, clopidol, florfenicol, sulfamethazine, sulfamethoxazole, sulfathiazole, tetracycline, tiamulin, tylosin)을 pH 6 McIlvaine buffer를 사용하여 아세트산 함유 아세토니트릴, $Na_2Cit.5H_2O$, $Na_3Cit.2H_2O$로 추출 후 $C_{18}$과 PSA로 정제하여 LC-MS/MS로 분석하는 모니터링을 수행하였다. 그 중 5종의 항생제 sulfamethazine, sulfathiazole, tylosin, tiamulin 및 clopidol이 국내 퇴액비 시료에서 검출되었으며 제안한 분석법은 퇴 액비 중 잔류 항생제 모니터링을 위한 빠르고 간편한 시험법이라 사료 된다. 본 실험을 통하여 퇴비 및 액비 중 축산 항생제의 잔류 현황을 파악하여 모니터링 자료를 확보하였고 이를 활용하여 검출된 항생제들이 안전한 토양 및 생태 환경 유지 및 관리의 기초 자료와 더불어 환경기준 예비 항목 및 설정(안)을 위한 기초자료로 제공 및 다양하게 활용될 수 있을 것으로 판단된다.

Keywords

References

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